Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 136, Issue 23, Pages 8269-8276Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja5006866
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Funding
- Center for Gas Separations Relevant to Clean Energy Technologies, an Energy Frontier Research Center (EFRC) - U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-SC0001015]
- Methane Opportunities for Vehicular Energy (MOVE) Program, an ARPA-E Project [DE-AR0000249]
- MOVE
- EFRC
- National Science Foundation [CHE-0911690, CMMI-0963509, CHE-0840518]
- Robert A. Welch Foundation [B-1542]
- U.S. DOE [DE-AC02-06CH11357]
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We demonstrate that rigidifying the structure of fluorescent linkers by structurally constraining them in metal-organic frameworks (MOFs) to control their conformation effectively tunes the fluorescence energy and enhances the quantum yield. Thus, a new tetraphenylethylene-based zirconium MOF exhibits a deep-blue fluorescent emission at 470 nm with a unity quantum yield (99.9 +/- 0.5%) under Ar, representing ca. 3600 cm(-1) blue shift and doubled radiative decay efficiency vs the linker precursor. An anomalous increase in the fluorescence lifetime and relative intensity takes place upon heating the solid MOF from cryogenic to ambient temperatures. The origin of these unusual photoluminescence properties is attributed to twisted linker conformation, intramolecular hindrance, and framework rigidity.
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